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Engineered cementitious composites (ECCs) are special types of fibre-reinforced cementitious composites (FRCC) with higher strain capacity which can be achieved with low fibre volume as low as 2% and total elimination of coarse aggregates. Due to the outstanding performance of ECCs, they are suitable for various construction and repair applications. However, in order for ECCs to achieve their properties; a high amount of binder which is primarily composed of Portland cement (PC) is used alongside a special type of ultrafine silica sand (USS) which is different from the conventional natural fine aggregates. The production of PC is known to be detrimental to the environment due to its high carbon dioxide emissions coupled with the high consumption of natural resources. Thus, the high use of PC content in ECCs posed a sustainability threat. Similarly, the USS used in ECCs are not readily available everywhere and are expensive. The processing of the USS coupled with its transportation over long distances would also increase the cost and embodied carbon of ECCs. Hence, in order to promote more development and applications of ECCs for various applications; this dissertation aims to provide innovative ways to improve the sustainability of ECCs and their performances. This dissertation offers four solutions to improve the sustainability of ECCs which are (i) use of unconventional industrial by-products as partial replacement of PC (ii) total replacement of PC in ECCs with alternative sustainable binders (iii) replacement of USS in ECCs with recycled materials and (iv) the use of supplementary cementitious materials to replace a high volume of PC. The findings from this study revealed sustainable ECCs with acceptable mechanical and durability performance can be achieved with the use of alternative binders or replacement of the conventional USS used in ECC mixtures. The sustainability and cost assessment of the ECCs indicated that the incorporation of industrial by-products such as blast furnace slag (BFS) especially at higher content is beneficial to reducing the negative environmental impact and economic burden associated with ECCs compared to the conventional ECC. The sustainability index and cost index of the ECCs further showed that the use of BFS is more beneficial when the sustainability and cost of the ECCs are compared with the corresponding performance. Similarly, the use of recycled materials as an alternative to USS was found to result in a significant reduction in the embodied carbon and cost of ECCs. The use of recycled materials such as expanded glass (EG) as aggregates in ECCs was also found to improve the thermal insulation properties of ECCs making such ECC suitable for the production of building envelope elements.

Engineered cementitious composites (ECCs) are special types of fibre-reinforced cementitious composites (FRCC) with higher strain capacity which can be achieved with low fibre volume as low as 2% and total elimination of coarse aggregates. Due to the outstanding performance of ECCs, they are suitable for various construction and repair applications. However, in order for ECCs to achieve their properties; a high amount of binder which is primarily composed of Portland cement (PC) is used alongside a special type of ultrafine silica sand (USS) which is different from the conventional natural fine aggregates. The production of PC is known to be detrimental to the environment due to its high carbon dioxide emissions coupled with the high consumption of natural resources. Thus, the high use of PC content in ECCs posed a sustainability threat. Similarly, the USS used in ECCs are not readily available everywhere and are expensive. The processing of the USS coupled with its transportation over long distances would also increase the cost and embodied carbon of ECCs. Hence, in order to promote more development and applications of ECCs for various applications; this dissertation aims to provide innovative ways to improve the sustainability of ECCs and their performances. This dissertation offers four solutions to improve the sustainability of ECCs which are (i) use of unconventional industrial by-products as partial replacement of PC (ii) total replacement of PC in ECCs with alternative sustainable binders (iii) replacement of USS in ECCs with recycled materials and (iv) the use of supplementary cementitious materials to replace a high volume of PC. The findings from this study revealed sustainable ECCs with acceptable mechanical and durability performance can be achieved with the use of alternative binders or replacement of the conventional USS used in ECC mixtures. The sustainability and cost assessment of the ECCs indicated that the incorporation of industrial by-products such as blast furnace slag (BFS) especially at higher content is beneficial to reducing the negative environmental impact and economic burden associated with ECCs compared to the conventional ECC. The sustainability index and cost index of the ECCs further showed that the use of BFS is more beneficial when the sustainability and cost of the ECCs are compared with the corresponding performance. Similarly, the use of recycled materials as an alternative to USS was found to result in a significant reduction in the embodied carbon and cost of ECCs. The use of recycled materials such as expanded glass (EG) as aggregates in ECCs was also found to improve the thermal insulation properties of ECCs making such ECC suitable for the production of building envelope elements.

II ABSTRACT Climate change is expected due to the increasing atmospheric concentrations of carbondioxide and other trace gasses, which lead to changes in the radioactive balance of the atmosphere. Such changes propagate further to those in temperature i and other climatic variables. Hydrologic systems and water resources are likely to be seriously impacted by global climate change. Such processes as surface runoff, precipitation, soil moisture, groundwater, water quality, and sea levels will be significantly exposed to effects of climate change. Eventually, these effects will have to be considered in water resources planning and management. The study presented stems from the above needs and addresses the problem of climate change-water resources interactions. It is intended here to investigate the possible effects of climate change on watershed scale hydrologic processes and water demand. Within this context, the current methods used in developed countries are applied to the case of the Gediz River Basin, and possible impacts of changes in climatic variables, i.e., precipitation and temperature, are investigated as they relate to runoff The results of the study should not considered as exact values to represent the effects of climate change. They are essentially `estimates` on `likely` effects of an expected climate change. However, the results also show that, if the prescribed climate change scenarios do occur in the future, they will have significant effects on the hydrology of the basin which, in turn, affects water demand for various water resources development plans. Accordingly, the study presented should be considered as an initial step towards assessment of climate change impacts and should be reaccomplished in future attempts towards any planning or management activity in the basin. ÖZET İklim değişikliği, atmosferdeki karbondioksit (CO2) ve diğer antropojen sera gazı konsantrasyonlarının giderek artması sonucu beklenmektedir. İklim değişikliğinin sonucunda beklenen en önemli olgu, sıcaklık, yağış, evapotranspirasyon, akış gibi temel iklimsel ve hidrolojik değişkenlerdeki muhtemel değişimlerdir. Bu etkilerin su kaynakları planlama ve yönetiminde değerlendirilmesi gerekmektedir. Sunulan çalışma, iklim değişikliğinin su kaynakları ile olan ilişkisini incelemektedir. Bu değişimlerden hidrolojik çevrimin ve su kaynaklarının gerek miktarı ve gerekse kalitesinin de etkilenmesi beklenmektedir. Dolayısıyla, küresel iklim değişikliğinin havza su dengesine ve su kaynaklarının planlama ve yönetimine de yansıması söz konusudur. Bu kapsamda sunulan çalışmada alt havza bazında sıcaklık ve yağış gibi iklim parametrelerinin, akıma olan etkileri incelenmiş ve duyarlılık analizi ile sonuçlar değerlendirilmiştir. 75

II ABSTRACT Climate change is expected due to the increasing atmospheric concentrations of carbondioxide and other trace gasses, which lead to changes in the radioactive balance of the atmosphere. Such changes propagate further to those in temperature i and other climatic variables. Hydrologic systems and water resources are likely to be seriously impacted by global climate change. Such processes as surface runoff, precipitation, soil moisture, groundwater, water quality, and sea levels will be significantly exposed to effects of climate change. Eventually, these effects will have to be considered in water resources planning and management. The study presented stems from the above needs and addresses the problem of climate change-water resources interactions. It is intended here to investigate the possible effects of climate change on watershed scale hydrologic processes and water demand. Within this context, the current methods used in developed countries are applied to the case of the Gediz River Basin, and possible impacts of changes in climatic variables, i.e., precipitation and temperature, are investigated as they relate to runoff The results of the study should not considered as exact values to represent the effects of climate change. They are essentially `estimates` on `likely` effects of an expected climate change. However, the results also show that, if the prescribed climate change scenarios do occur in the future, they will have significant effects on the hydrology of the basin which, in turn, affects water demand for various water resources development plans. Accordingly, the study presented should be considered as an initial step towards assessment of climate change impacts and should be reaccomplished in future attempts towards any planning or management activity in the basin. ÖZET İklim değişikliği, atmosferdeki karbondioksit (CO2) ve diğer antropojen sera gazı konsantrasyonlarının giderek artması sonucu beklenmektedir. İklim değişikliğinin sonucunda beklenen en önemli olgu, sıcaklık, yağış, evapotranspirasyon, akış gibi temel iklimsel ve hidrolojik değişkenlerdeki muhtemel değişimlerdir. Bu etkilerin su kaynakları planlama ve yönetiminde değerlendirilmesi gerekmektedir. Sunulan çalışma, iklim değişikliğinin su kaynakları ile olan ilişkisini incelemektedir. Bu değişimlerden hidrolojik çevrimin ve su kaynaklarının gerek miktarı ve gerekse kalitesinin de etkilenmesi beklenmektedir. Dolayısıyla, küresel iklim değişikliğinin havza su dengesine ve su kaynaklarının planlama ve yönetimine de yansıması söz konusudur. Bu kapsamda sunulan çalışmada alt havza bazında sıcaklık ve yağış gibi iklim parametrelerinin, akıma olan etkileri incelenmiş ve duyarlılık analizi ile sonuçlar değerlendirilmiştir. 75

In recent decades, many societal changes have unfolded, including population ageing, reconfigurations of household structures, labour market transformation, and a secular deceleration of economic growth. These shifts pose considerable challenges to preexisting welfare states, particularly to the efficacy of countries’ pension systems. This dissertation examines the context and trajectory of pension reforms in Mexico, the United Kingdom, and the United States. Its contribution is to ascertain the viability and political feasibility of reforms that enhance the financial sustainability of their pension systems, while maintaining adequate income and coverage levels. The dissertation builds on political economy approaches and on the institutionalist literature, which highlight how the role of interest groups and structure of institutions and political systems shape policy outcomes. The frameworks of blame avoidance and credit-claiming are also considered, to provide a comprehensive analysis of the complex dynamics surrounding pension systems and reform efforts. This dissertation uses a mixed-methods approach – including public opinion surveys of 3,000+ individuals, semi-structured elite interviews, historical document analyses, and specialized fiscal and actuarial projections of selected pension reforms in the three selected countries. It addresses three core research questions: 1) What is the current context for pension reform in Mexico, the United Kingdom, and the United States given their histories? 2) Is the necessary (for achieving specific minimum levels of sustainability, adequacy, and coverage) pension reform politically feasible? 3) How do the characteristics of each reform affect its political feasibility? Corollary: The modification of which channel (benefits, contributions, retirement age) is perceived as more politically feasible for diverse stakeholders? The methodology chosen provides a timely picture of the context surrounding potential pension reforms in the three case studies. In Mexico, credit-claiming and the interests of private stakeholders explain the success of recent pension reforms, and partisan politics are the key determinants for future fiscal changes. For the United Kingdom, the institutionalist literature helps explain the reasons for the relatively easier reform avenues; the most politically feasible reforms are those in the private sector, while the housing market is of key importance for pensions. In the United States, the institutionalist literature and the framework of blame avoidance also help explain the current legislative gridlock and the reasons why no major reform has been enacted for decades. For Mexico and the United Kingdom there exist politically feasible reforms, notably a modification of the retirement age channel, that can increase the system’s sustainability while maintaining income adequacy and coverage; whereas based on the current context of extreme polarisation and legislative gridlock, there do not seem to exist politically feasible pension reforms that preserve the structure of Social Security in the United States. The dissertation brings the lens of political feasibility to bear on a previously technical literature on the structure of the pension systems in the three countries, and thus on the feasibility of reform to deliver financial sustainability, adequacy of retirement incomes, and adequate coverage of the old age population. It identifies the feasible routes for reform in Mexico and the United Kingdom, but concludes that the political economy context the United States has reached rules out feasible reforms of its current pension structures.

In recent decades, many societal changes have unfolded, including population ageing, reconfigurations of household structures, labour market transformation, and a secular deceleration of economic growth. These shifts pose considerable challenges to preexisting welfare states, particularly to the efficacy of countries’ pension systems. This dissertation examines the context and trajectory of pension reforms in Mexico, the United Kingdom, and the United States. Its contribution is to ascertain the viability and political feasibility of reforms that enhance the financial sustainability of their pension systems, while maintaining adequate income and coverage levels. The dissertation builds on political economy approaches and on the institutionalist literature, which highlight how the role of interest groups and structure of institutions and political systems shape policy outcomes. The frameworks of blame avoidance and credit-claiming are also considered, to provide a comprehensive analysis of the complex dynamics surrounding pension systems and reform efforts. This dissertation uses a mixed-methods approach – including public opinion surveys of 3,000+ individuals, semi-structured elite interviews, historical document analyses, and specialized fiscal and actuarial projections of selected pension reforms in the three selected countries. It addresses three core research questions: 1) What is the current context for pension reform in Mexico, the United Kingdom, and the United States given their histories? 2) Is the necessary (for achieving specific minimum levels of sustainability, adequacy, and coverage) pension reform politically feasible? 3) How do the characteristics of each reform affect its political feasibility? Corollary: The modification of which channel (benefits, contributions, retirement age) is perceived as more politically feasible for diverse stakeholders? The methodology chosen provides a timely picture of the context surrounding potential pension reforms in the three case studies. In Mexico, credit-claiming and the interests of private stakeholders explain the success of recent pension reforms, and partisan politics are the key determinants for future fiscal changes. For the United Kingdom, the institutionalist literature helps explain the reasons for the relatively easier reform avenues; the most politically feasible reforms are those in the private sector, while the housing market is of key importance for pensions. In the United States, the institutionalist literature and the framework of blame avoidance also help explain the current legislative gridlock and the reasons why no major reform has been enacted for decades. For Mexico and the United Kingdom there exist politically feasible reforms, notably a modification of the retirement age channel, that can increase the system’s sustainability while maintaining income adequacy and coverage; whereas based on the current context of extreme polarisation and legislative gridlock, there do not seem to exist politically feasible pension reforms that preserve the structure of Social Security in the United States. The dissertation brings the lens of political feasibility to bear on a previously technical literature on the structure of the pension systems in the three countries, and thus on the feasibility of reform to deliver financial sustainability, adequacy of retirement incomes, and adequate coverage of the old age population. It identifies the feasible routes for reform in Mexico and the United Kingdom, but concludes that the political economy context the United States has reached rules out feasible reforms of its current pension structures.

The aggravating global problems of energy crisis, rising atmospheric greenhouse gas concentrations and accumulation of persistent waste have attracted the attention of scientists, policy-makers and global organisations to come up with effective and expeditious solutions to address these challenges. In this context, the development of sustainable technologies driven by renewable energy sources for the production of clean fuels and commodity chemicals from diverse waste feedstocks is an appealing approach towards creating a circular economy. Over the years, semiconductor photocatalysts based on TiO₂, CdS, carbon-nitrides (CNx) and carbon dots (CDs) have been widely used for the photocatalytic reforming (PC reforming) of pre-treated waste substrates to organic products, accompanied with clean hydrogen (H₂) generation. However, these conventional solar-driven processes suffer from major drawbacks such as low production rates, poor product selectivity, CO₂ release, challenging process and catalyst optimisation, and harsh waste pre-treatment conditions, which limit their commercial applicability. These challenges are tackled in this thesis with the introduction of new and efficient photoelectrochemical (PEC) and chemoenzymatic processes for reforming a diverse range of waste feedstocks to sustainable fuels. Solar-driven PEC reforming based on halide perovskite light-absorber is first developed as an attractive alternative to PC reforming. The PEC systems consist of a perovskite|Pt photocathode for clean H₂ production and a Cu-Pd alloy anode for reforming diverse waste streams, including pre-treated cellulosic biomass, polyethylene terephthalate (PET) plastics, and industrial by-product glycerol into industrially-relevant, value-added chemicals (gluconic acid, glycolic acid and glyceric acid) without any externally applied bias or voltage. Additionally, the single light-absorber PEC systems can also convert the airborne waste stream and greenhouse gas CO₂ to diverse products with the simultaneous reforming of PET plastics with no applied voltage. The perovskite-based photocathode enables the integration of different CO₂ reduction catalysts such as a molecular cobalt porphyrin, a Cu-In alloy and formate dehydrogenase enzyme, which produce CO, syngas and formate, respectively. The versatile PEC systems, which can be assembled in either a ‘two-compartment’ or standalone ‘artificial leaf’ configurations achieve 60‒90% oxidation product selectivity (with no over-oxidation) and >100 µmol cm‾² h‾¹ product formation rates, corresponding to 10²‒10⁴ times higher activity than conventional PC reforming systems. In addition to developing PEC platforms, this thesis also explores avenues for circumventing the harsh alkaline pre-treatment strategies (pH >13, 60‒80 ºC) adopted for photoreforming waste substrates. For this purpose, a chemoenzymatic pathway is introduced whereby PET and polycaprolactone plastics were deconstructed using functional enzymes under benign conditions (pH 6‒8, 37‒65 ºC), followed by PC reforming using Pt loaded TiO₂ (TiO₂|Pt) or Ni₂P loaded carbon-nitride (CNx|Ni₂P) photocatalysts. The chemoenzymatic reforming process demonstrates versatility in upcycling polyester films and nanoplastics for H₂ production at high yields reaching ∼10³‒10⁴ µmol gsub‾¹ and activities at >500 µmol gcat‾¹ h‾¹. The utilisation of enzyme pre-treated plastics also allowed the coupling of plastic reforming with photocatalytic CO₂-to-syngas conversion using a phosphonated cobalt bis(terpyridine) co-catalyst immobilised on TiO₂ (TiO₂|CotpyP). Finally, moving beyond solar-driven systems, a bio-electrocatalytic flow process is demonstrated for the conversion of microbe pre-treated food waste to ethylene (an important feedstock in the chemical industry) on graphitic carbon electrodes via succinic acid as the central intermediate. In conclusion, with its focus on improving efficiencies, achieving selective product formation, building versatile platforms, diversifying substrate and product scope, and reducing carbon footprint and economic strain, this thesis aims to bring sustainable waste-to-fuel technologies a step closer to commercial implementation.

The aggravating global problems of energy crisis, rising atmospheric greenhouse gas concentrations and accumulation of persistent waste have attracted the attention of scientists, policy-makers and global organisations to come up with effective and expeditious solutions to address these challenges. In this context, the development of sustainable technologies driven by renewable energy sources for the production of clean fuels and commodity chemicals from diverse waste feedstocks is an appealing approach towards creating a circular economy. Over the years, semiconductor photocatalysts based on TiO₂, CdS, carbon-nitrides (CNx) and carbon dots (CDs) have been widely used for the photocatalytic reforming (PC reforming) of pre-treated waste substrates to organic products, accompanied with clean hydrogen (H₂) generation. However, these conventional solar-driven processes suffer from major drawbacks such as low production rates, poor product selectivity, CO₂ release, challenging process and catalyst optimisation, and harsh waste pre-treatment conditions, which limit their commercial applicability. These challenges are tackled in this thesis with the introduction of new and efficient photoelectrochemical (PEC) and chemoenzymatic processes for reforming a diverse range of waste feedstocks to sustainable fuels. Solar-driven PEC reforming based on halide perovskite light-absorber is first developed as an attractive alternative to PC reforming. The PEC systems consist of a perovskite|Pt photocathode for clean H₂ production and a Cu-Pd alloy anode for reforming diverse waste streams, including pre-treated cellulosic biomass, polyethylene terephthalate (PET) plastics, and industrial by-product glycerol into industrially-relevant, value-added chemicals (gluconic acid, glycolic acid and glyceric acid) without any externally applied bias or voltage. Additionally, the single light-absorber PEC systems can also convert the airborne waste stream and greenhouse gas CO₂ to diverse products with the simultaneous reforming of PET plastics with no applied voltage. The perovskite-based photocathode enables the integration of different CO₂ reduction catalysts such as a molecular cobalt porphyrin, a Cu-In alloy and formate dehydrogenase enzyme, which produce CO, syngas and formate, respectively. The versatile PEC systems, which can be assembled in either a ‘two-compartment’ or standalone ‘artificial leaf’ configurations achieve 60‒90% oxidation product selectivity (with no over-oxidation) and >100 µmol cm‾² h‾¹ product formation rates, corresponding to 10²‒10⁴ times higher activity than conventional PC reforming systems. In addition to developing PEC platforms, this thesis also explores avenues for circumventing the harsh alkaline pre-treatment strategies (pH >13, 60‒80 ºC) adopted for photoreforming waste substrates. For this purpose, a chemoenzymatic pathway is introduced whereby PET and polycaprolactone plastics were deconstructed using functional enzymes under benign conditions (pH 6‒8, 37‒65 ºC), followed by PC reforming using Pt loaded TiO₂ (TiO₂|Pt) or Ni₂P loaded carbon-nitride (CNx|Ni₂P) photocatalysts. The chemoenzymatic reforming process demonstrates versatility in upcycling polyester films and nanoplastics for H₂ production at high yields reaching ∼10³‒10⁴ µmol gsub‾¹ and activities at >500 µmol gcat‾¹ h‾¹. The utilisation of enzyme pre-treated plastics also allowed the coupling of plastic reforming with photocatalytic CO₂-to-syngas conversion using a phosphonated cobalt bis(terpyridine) co-catalyst immobilised on TiO₂ (TiO₂|CotpyP). Finally, moving beyond solar-driven systems, a bio-electrocatalytic flow process is demonstrated for the conversion of microbe pre-treated food waste to ethylene (an important feedstock in the chemical industry) on graphitic carbon electrodes via succinic acid as the central intermediate. In conclusion, with its focus on improving efficiencies, achieving selective product formation, building versatile platforms, diversifying substrate and product scope, and reducing carbon footprint and economic strain, this thesis aims to bring sustainable waste-to-fuel technologies a step closer to commercial implementation.

Ammonia has been responsible for feeding population growth in the 20th century through synthetic fertilizer, and is poised to become the preferred energy storage medium for a society powered by renewable electricity in the 21st century. However, conventional brown ammonia production through the Haber-Bosch process is optimized for utilization of centralized and steady energy supply from fossil-fuels. When shifting to distributed and intermittent energy supply through wind and solar energy, a re-optimization is required for a low-capital and flexible green ammonia production processes. This thesis re-designs and Haber-Bosch process by targeting the integration of reaction and separation in a single process vessel at low pressures, thereby achieving the simplification and down-scaling of the high pressure recycle loop of the Haber-Bosch process. Materials are developed for this purpose, the feasibility of integration is demonstrated, and mathematical modeling is utilized for assessing the application of the single-vessel process to a range of renewable energy sources in comparison to competing ammonia production processes. Herein, a catalyst with low-temperature (< 350°C) and high-conversion (i.e. near equilibrium) activity is developed using ruthenium nanoparticles as the active metal supported on ceria and promoted with cesium to mitigate hydrogen and ammonia inhibition, respectively. This catalyst is compared to commercial iron-based catalyst from the perspective of the final application. Concurrently, a high-temperature (> 300°C) manganese chloride absorbent is developed that resists decomposition and is stable when supported on silica. These catalyst and absorbent are integrated in a layered reactor configuration to demonstrate the feasibility of the integrated process by exceeding single-pass reaction equilibrium. Mathematical modelling of ammonia production processes illustrates that at small-scales (< 1 t day-1) the single-vessel process is optimal compared to the Haber-Bosch process due to its modular design. In addition, it can achieve simpler ramping because the Haber-Bosch process is constrained by heat-integration in the recycle loop and the potential for runaway reaction. For final application, the pairing of ammonia production processes with examples of intermittent solar and wind sources demonstrates that the flexibility of the production process is essential when considering non-ideal sources of energy with a long-term (e.g. seasonal) oscillations. Flexible ammonia production also expands the economic usage of ammonia as an energy storage vector from the seasonal to the weekly time-scale, with advantage compared to batteries or hydrogen. The work of this thesis provides a framework for advancing the electrification of the chemical industry given the novel constrains of intermittent and distributed renewable energy. A systems level approach is applied from the ground up, starting from material design and progressing to optimized process design and application.

Ammonia has been responsible for feeding population growth in the 20th century through synthetic fertilizer, and is poised to become the preferred energy storage medium for a society powered by renewable electricity in the 21st century. However, conventional brown ammonia production through the Haber-Bosch process is optimized for utilization of centralized and steady energy supply from fossil-fuels. When shifting to distributed and intermittent energy supply through wind and solar energy, a re-optimization is required for a low-capital and flexible green ammonia production processes. This thesis re-designs and Haber-Bosch process by targeting the integration of reaction and separation in a single process vessel at low pressures, thereby achieving the simplification and down-scaling of the high pressure recycle loop of the Haber-Bosch process. Materials are developed for this purpose, the feasibility of integration is demonstrated, and mathematical modeling is utilized for assessing the application of the single-vessel process to a range of renewable energy sources in comparison to competing ammonia production processes. Herein, a catalyst with low-temperature (< 350°C) and high-conversion (i.e. near equilibrium) activity is developed using ruthenium nanoparticles as the active metal supported on ceria and promoted with cesium to mitigate hydrogen and ammonia inhibition, respectively. This catalyst is compared to commercial iron-based catalyst from the perspective of the final application. Concurrently, a high-temperature (> 300°C) manganese chloride absorbent is developed that resists decomposition and is stable when supported on silica. These catalyst and absorbent are integrated in a layered reactor configuration to demonstrate the feasibility of the integrated process by exceeding single-pass reaction equilibrium. Mathematical modelling of ammonia production processes illustrates that at small-scales (< 1 t day-1) the single-vessel process is optimal compared to the Haber-Bosch process due to its modular design. In addition, it can achieve simpler ramping because the Haber-Bosch process is constrained by heat-integration in the recycle loop and the potential for runaway reaction. For final application, the pairing of ammonia production processes with examples of intermittent solar and wind sources demonstrates that the flexibility of the production process is essential when considering non-ideal sources of energy with a long-term (e.g. seasonal) oscillations. Flexible ammonia production also expands the economic usage of ammonia as an energy storage vector from the seasonal to the weekly time-scale, with advantage compared to batteries or hydrogen. The work of this thesis provides a framework for advancing the electrification of the chemical industry given the novel constrains of intermittent and distributed renewable energy. A systems level approach is applied from the ground up, starting from material design and progressing to optimized process design and application.